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Abstract <p>Despite being an excellent candidate for a photocathode, Cu<sub>2</sub>ZnSnS<sub>4</sub> (CZTS) performance is limited by suboptimal bulk and interfacial charge carrier dynamics. In this work, we introduce a facile and versatile CZTS precursor seed layer engineering technique, which significantly enhances crystal growth and mitigates detrimental defects in the post-sulfurized CZTS light-absorbing films. This effective optimization of defects and charge carrier dynamics results in a highly efficient CZTS/CdS/TiO<sub>2</sub>/Pt thin-film photocathode, achieving a record half-cell solar-to-hydrogen (HC-STH) conversion efficiency of 9.91%. Additionally, the photocathode exhibits a highest photocurrent density (<i>J</i><sub>ph</sub>) of 29.44&#xa0;mA&#xa0;cm<sup>−2</sup> (at 0 <i>V</i><sub>RHE</sub>) and favorable onset potential (<i>V</i><sub>on</sub>) of 0.73 <i>V</i><sub>RHE</sub>. Furthermore, our CTZS photocathode demonstrates a remarkable <i>J</i><sub>ph</sub> of 16.54&#xa0;mA&#xa0;cm<sup>−2</sup> and HC-STH efficiency of 2.56% in natural seawater, followed by an impressive unbiased STH efficiency of 2.20% in a CZTS-BiVO<sub>4</sub> tandem cell. The scalability of this approach is underscored by the successful fabrication of a 4 × 4 cm<sup>2</sup> module, highlighting its significant potential for practical, unbiased in situ solar seawater splitting applications.</p>

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Highest Solar-to-Hydrogen Conversion Efficiency in Cu2ZnSnS4 Photocathodes and Its Directly Unbiased Solar Seawater Splitting

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年5月16日

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  • Muhammad Abbas,
  • Shuo Chen,
  • Zhidong Li,
  • Muhammad Ishaq,
  • Zhuanghao Zheng,
  • Juguang Hu,
  • Zhenghua Su,
  • Yanbo Li,
  • Liming Ding,
  • Guangxing Liang

摘要

Abstract

Despite being an excellent candidate for a photocathode, Cu2ZnSnS4 (CZTS) performance is limited by suboptimal bulk and interfacial charge carrier dynamics. In this work, we introduce a facile and versatile CZTS precursor seed layer engineering technique, which significantly enhances crystal growth and mitigates detrimental defects in the post-sulfurized CZTS light-absorbing films. This effective optimization of defects and charge carrier dynamics results in a highly efficient CZTS/CdS/TiO2/Pt thin-film photocathode, achieving a record half-cell solar-to-hydrogen (HC-STH) conversion efficiency of 9.91%. Additionally, the photocathode exhibits a highest photocurrent density (Jph) of 29.44 mA cm−2 (at 0 VRHE) and favorable onset potential (Von) of 0.73 VRHE. Furthermore, our CTZS photocathode demonstrates a remarkable Jph of 16.54 mA cm−2 and HC-STH efficiency of 2.56% in natural seawater, followed by an impressive unbiased STH efficiency of 2.20% in a CZTS-BiVO4 tandem cell. The scalability of this approach is underscored by the successful fabrication of a 4 × 4 cm2 module, highlighting its significant potential for practical, unbiased in situ solar seawater splitting applications.